Julie Beth Zimmerman, Gregory Lowry, Fernando Rosario-Ortiz, Paul Westerhoff, Daniel Alessi, Pedro Alvarez, Alexandra Boehm, Ian Cousins, Jordi Dachs, Matthew Eckelman, Imad El Haddad, Pablo Gago-Ferrero, Jorge Gardea-Torresdey, Jacqueline MacDonald Gibson, Keri Hornbuckle, Heileen Hsu-Kim, Juliane Hollender, Atsuko Ikeda, Frederic Leusch, Melissa Maurer-Jones, James Mihelcic, Shelly Miller, Lutgarde Raskin, Z. Jason Ren, Susan Richardson, Daniel Schlenk, Huahong Shi, Paul Tratnyek, David Waite, Shuxiao Wang, Zhanyun Wang, Michael Wong, Sukhwan Yoon
There is an old saying that “facts do not need you to believe them to be true”. This has never been more relevant. In an era where scientific research, particularly in environmental, health, and climate science, faces mounting political challenges, we must reaffirm that our work is not contingent on ideology but on the immutable laws of nature. A molecule of carbon dioxide does not recognize political debates over international climate agreements. It will, however, contribute to climate change because of the fundamental physics governing the carbon–oxygen double bond. A molecule of methylene chloride does not consider economic arguments about regulatory limits, yet it will still be capable of causing cancer when it enters the human body. Per- and polyfluoroalkyl substances, PCBs, pesticides, and heavy metals do not change their toxicity based on geopolitical preferences. The virulence of a pathogen is not determined by socially acceptable risk standards. The dangers these and other substances and organisms pose are dictated by their physical and chemical properties, indifferent to political rhetoric, economic debates, or national borders. Science-based environmental policies have delivered tangible benefits. The United States’ Clean Water and Air Acts dramatically improved water and air quality, preventing disease and mortality while saving billions in healthcare costs. Many countries use the World Health Organization’s health-based drinking water quality standards as the basis for their own national standards, which have significantly reduced infant mortality from infectious diseases. The Montreal Protocol has meaningfully benefited the planet by protecting the ozone layer and mitigating climate change. Multilateral agreements such as the Stockholm Convention on Persistent Organic Pollutants and the Minamata Convention on mercury have curtailed our exposure to hazardous chemicals. China’s clean air action plans have achieved remarkable air quality improvements in record time, demonstrating that environmental progress is possible even amid rapid economic expansion. Today’s environmental crises continue to defy geopolitical boundaries and the politics that compound them. Mercury pollution in tuna, plastics in the ocean, and chemical contaminants in Arctic and Antarctic wildlife are a few examples illustrating that no single country or continent can confront these challenges alone. The increasing frequency and intensity of environmental disasters due to climate change, from record-breaking wildfires to catastrophic flooding, further underscore the urgency for global, coordinated actions. As environmental scientists and engineers, our mandate is clear: we must remain steadfast in our commitment to truth and scientific integrity. We must amplify our voices, educating, informing, and engaging with decision-makers and the public and insisting that scientific facts underpin policy decisions. More than ever, it is crucial to share our findings effectivel
{"title":"Apolitical Science","authors":"Julie Beth Zimmerman, Gregory Lowry, Fernando Rosario-Ortiz, Paul Westerhoff, Daniel Alessi, Pedro Alvarez, Alexandra Boehm, Ian Cousins, Jordi Dachs, Matthew Eckelman, Imad El Haddad, Pablo Gago-Ferrero, Jorge Gardea-Torresdey, Jacqueline MacDonald Gibson, Keri Hornbuckle, Heileen Hsu-Kim, Juliane Hollender, Atsuko Ikeda, Frederic Leusch, Melissa Maurer-Jones, James Mihelcic, Shelly Miller, Lutgarde Raskin, Z. Jason Ren, Susan Richardson, Daniel Schlenk, Huahong Shi, Paul Tratnyek, David Waite, Shuxiao Wang, Zhanyun Wang, Michael Wong, Sukhwan Yoon","doi":"10.1021/acs.est.5c03696","DOIUrl":"https://doi.org/10.1021/acs.est.5c03696","url":null,"abstract":"There is an old saying that “facts do not need you to believe them to be true”. This has never been more relevant. In an era where scientific research, particularly in environmental, health, and climate science, faces mounting political challenges, we must reaffirm that our work is not contingent on ideology but on the immutable laws of nature. A molecule of carbon dioxide does not recognize political debates over international climate agreements. It will, however, contribute to climate change because of the fundamental physics governing the carbon–oxygen double bond. A molecule of methylene chloride does not consider economic arguments about regulatory limits, yet it will still be capable of causing cancer when it enters the human body. Per- and polyfluoroalkyl substances, PCBs, pesticides, and heavy metals do not change their toxicity based on geopolitical preferences. The virulence of a pathogen is not determined by socially acceptable risk standards. The dangers these and other substances and organisms pose are dictated by their physical and chemical properties, indifferent to political rhetoric, economic debates, or national borders. Science-based environmental policies have delivered tangible benefits. The United States’ Clean Water and Air Acts dramatically improved water and air quality, preventing disease and mortality while saving billions in healthcare costs. Many countries use the World Health Organization’s health-based drinking water quality standards as the basis for their own national standards, which have significantly reduced infant mortality from infectious diseases. The Montreal Protocol has meaningfully benefited the planet by protecting the ozone layer and mitigating climate change. Multilateral agreements such as the Stockholm Convention on Persistent Organic Pollutants and the Minamata Convention on mercury have curtailed our exposure to hazardous chemicals. China’s clean air action plans have achieved remarkable air quality improvements in record time, demonstrating that environmental progress is possible even amid rapid economic expansion. Today’s environmental crises continue to defy geopolitical boundaries and the politics that compound them. Mercury pollution in tuna, plastics in the ocean, and chemical contaminants in Arctic and Antarctic wildlife are a few examples illustrating that no single country or continent can confront these challenges alone. The increasing frequency and intensity of environmental disasters due to climate change, from record-breaking wildfires to catastrophic flooding, further underscore the urgency for global, coordinated actions. As environmental scientists and engineers, our mandate is clear: we must remain steadfast in our commitment to truth and scientific integrity. We must amplify our voices, educating, informing, and engaging with decision-makers and the public and insisting that scientific facts underpin policy decisions. More than ever, it is crucial to share our findings effectivel","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"1 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798315","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pranav Nair, Holly Barrett, Kaylin Tanoto, Linna Xie, Jianxian Sun, Diwen Yang, Han Yao, Datong Song, Hui Peng
Distinct from other nontoxic phenyl-p-phenylenediamine (PPD) quinones, N-(1,3-dimethylbutyl)-N′-phenyl-p-phenylenediamine-quinone (6PPD-Q) was recently discovered to be regioselectively metabolized to alkyl hydroxylated metabolites (alkyl–OH-6PPD-Q) in rainbow trout. It remains unknown whether the unique alkyl–OH-6PPD-Q contributes to the toxicity of 6PPD-Q. To test this, we herein synthesized chemical standards of alkyl–OH-6PPD-Q isomers and investigated their metabolic formation mechanism and toxicity. The predominant alkyl–OH-6PPD-Q was confirmed to be hydroxylated on the C4 tertiary carbon (C4–OH-6PPD-Q). The formation of C4–OH-6PPD-Q was only observed in microsomal but not in cytosolic fractions of rainbow trout (O. mykiss) liver S9. A general cytochrome P450 (CYP450) inhibitor fluoxetine inhibited the formation of hydroxylated metabolites of 6PPD-Q, supporting that CYP450 catalyzed the hydroxylation. This well-explained the compound- and regio-selective formation of C4–OH-6PPD-Q, due to the weak C–H bond on the C4 tertiary carbon. Surprisingly, while cytotoxicity was observed for 6PPD-Q and C3–OH-6PPD-Q in a coho salmon (O. kisutch) embryo (CSE-119) cell line, no toxicity was observed for C4–OH-6PPD-Q. To further confirm this under physiologically relevant conditions, we fractionated 6PPD-Q metabolites formed in the liver microsome of rainbow trout. Cytotoxicity was observed for the fraction of 6PPD-Q, but not the fraction of C4–OH-6PPD-Q. In summary, this study highlighted the C4 tertiary carbon as the key moiety for both metabolism and toxicity of 6PPD-Q and confirmed that alkyl hydroxylation is a detoxification pathway for 6PPD-Q.
{"title":"Structure and Toxicity Characterization of Alkyl Hydroxylated Metabolites of 6PPD-Q","authors":"Pranav Nair, Holly Barrett, Kaylin Tanoto, Linna Xie, Jianxian Sun, Diwen Yang, Han Yao, Datong Song, Hui Peng","doi":"10.1021/acs.est.4c11823","DOIUrl":"https://doi.org/10.1021/acs.est.4c11823","url":null,"abstract":"Distinct from other nontoxic phenyl-<i>p</i>-phenylenediamine (PPD) quinones, <i>N</i>-(1,3-dimethylbutyl)-<i>N</i>′-phenyl-<i>p</i>-phenylenediamine-quinone (6PPD-Q) was recently discovered to be regioselectively metabolized to alkyl hydroxylated metabolites (alkyl–OH-6PPD-Q) in rainbow trout. It remains unknown whether the unique alkyl–OH-6PPD-Q contributes to the toxicity of 6PPD-Q. To test this, we herein synthesized chemical standards of alkyl–OH-6PPD-Q isomers and investigated their metabolic formation mechanism and toxicity. The predominant alkyl–OH-6PPD-Q was confirmed to be hydroxylated on the C<sub>4</sub> tertiary carbon (C<sub>4</sub>–OH-6PPD-Q). The formation of C<sub>4</sub>–OH-6PPD-Q was only observed in microsomal but not in cytosolic fractions of rainbow trout (<i>O. mykiss</i>) liver S9. A general cytochrome P450 (CYP450) inhibitor fluoxetine inhibited the formation of hydroxylated metabolites of 6PPD-Q, supporting that CYP450 catalyzed the hydroxylation. This well-explained the compound- and regio-selective formation of C<sub>4</sub>–OH-6PPD-Q, due to the weak C–H bond on the C<sub>4</sub> tertiary carbon. Surprisingly, while cytotoxicity was observed for 6PPD-Q and C<sub>3</sub>–OH-6PPD-Q in a coho salmon (<i>O. kisutch</i>) embryo (CSE-119) cell line, no toxicity was observed for C<sub>4</sub>–OH-6PPD-Q. To further confirm this under physiologically relevant conditions, we fractionated 6PPD-Q metabolites formed in the liver microsome of rainbow trout. Cytotoxicity was observed for the fraction of 6PPD-Q, but not the fraction of C<sub>4</sub>–OH-6PPD-Q. In summary, this study highlighted the C<sub>4</sub> tertiary carbon as the key moiety for both metabolism and toxicity of 6PPD-Q and confirmed that alkyl hydroxylation is a detoxification pathway for 6PPD-Q.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"244 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798193","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pablo A. Lara-Martín, Lena Schinkel, Yves Eberhard, Walter Giger, Michael Berg, Juliane Hollender
The increasing amount of sewage sludge generated during wastewater treatment poses both growing management challenge and environmental issues. Sludge with many co-occurring contaminants is often destined to land application which raises concern regarding human and environmental health. It is also a good integrator in time and space and can provide valuable information on consumption pattern and change over time. Here, we have conducted suspect and nontarget screening (SNTS) in sludge from 29 wastewater treatment plants (WWTPs) covering 30% of the Swiss population. Over 500 contaminants were identified and up to 382 quantified, with concentrations ranging from a few ng/g to several thousand ng/g, which translated into total annual loads of approximately 5 g of micropollutants per Swiss citizen. The distribution of detected substances was dominated by pharmaceuticals in terms of number of compounds (>250) and personal care products in terms of concentration (e.g., 75 μg/g for linoleic acid). Homologous series analysis revealed the presence of multiple classes of surfactants among those compounds with the highest signal intensities in sludge. Principal component analysis and hierarchical clustering showed that spatial distribution of contaminants across Switzerland was not homogeneous, while Pearson correlation indicated that changes can be attributed to different anaerobic digestion times in WWTPs.
{"title":"Suspect and Nontarget Screening of Organic Micropollutants in Swiss Sewage Sludge: A Nationwide Survey","authors":"Pablo A. Lara-Martín, Lena Schinkel, Yves Eberhard, Walter Giger, Michael Berg, Juliane Hollender","doi":"10.1021/acs.est.4c13217","DOIUrl":"https://doi.org/10.1021/acs.est.4c13217","url":null,"abstract":"The increasing amount of sewage sludge generated during wastewater treatment poses both growing management challenge and environmental issues. Sludge with many co-occurring contaminants is often destined to land application which raises concern regarding human and environmental health. It is also a good integrator in time and space and can provide valuable information on consumption pattern and change over time. Here, we have conducted suspect and nontarget screening (SNTS) in sludge from 29 wastewater treatment plants (WWTPs) covering 30% of the Swiss population. Over 500 contaminants were identified and up to 382 quantified, with concentrations ranging from a few ng/g to several thousand ng/g, which translated into total annual loads of approximately 5 g of micropollutants per Swiss citizen. The distribution of detected substances was dominated by pharmaceuticals in terms of number of compounds (>250) and personal care products in terms of concentration (e.g., 75 μg/g for linoleic acid). Homologous series analysis revealed the presence of multiple classes of surfactants among those compounds with the highest signal intensities in sludge. Principal component analysis and hierarchical clustering showed that spatial distribution of contaminants across Switzerland was not homogeneous, while Pearson correlation indicated that changes can be attributed to different anaerobic digestion times in WWTPs.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"36 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798196","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pranav Nair, Jianxian Sun, Linna Xie, Lisa Kennedy, Derek Kozakiewicz, Sonya M. Kleywegt, Chunyan Hao, Hannah Byun, Holly Barrett, Joshua Baker, Joseph Monaghan, Erik T. Krogh, Datong Song, Hui Peng
N-(1,3-Dimethylbutyl)-N′-phenyl-p-phenylenediamine-quinone (6PPD-Q), the tire rubber-derived transformation product of 6PPD, was recently discovered to cause the acute mortality of coho salmon (Oncorhynchus kisutch). Aiming to identify potential replacement antiozonants for 6PPD that do not produce toxic quinones, seven PPD-quinones with distinct side chains were synthesized to investigate their structure-related toxicities in vivo using rainbow trout (Oncorhynchus mykiss). While 6PPD-Q exerted high toxicity (96 h LC50 = 0.35 μg/L), toxicity was not observed for six other PPD-quinones despite their similar structures. The fish tissue concentrations of 6PPD-Q after sublethal exposure (0.29 μg/L) were comparable to the other PPD-quinones, which indicated that bioaccumulation levels were not the reason for the selective toxicity of 6PPD-Q. Hydroxylated PPD-quinones were detected as the predominant metabolites in fish tissue. Interestingly, a single major aromatic hydroxylation metabolite was detected for the alternate PPD-quinones, but two abundant OH-6PPD-Q isomers were detected for 6PPD-Q. MS2 spectra confirmed that hydroxylation occurred on the alkyl side chain for one isomer. The structurally selective toxicity of 6PPD-Q was also observed in a coho salmon (CSE-119) cell line, which further supports its intrinsic toxicity. This study reported the selective toxicity of 6PPD-Q and pinpointed the possibility for other PPDs to be applied as potential substitutes of 6PPD.
{"title":"Synthesis and Toxicity Evaluation of p-Phenylenediamine-Quinones","authors":"Pranav Nair, Jianxian Sun, Linna Xie, Lisa Kennedy, Derek Kozakiewicz, Sonya M. Kleywegt, Chunyan Hao, Hannah Byun, Holly Barrett, Joshua Baker, Joseph Monaghan, Erik T. Krogh, Datong Song, Hui Peng","doi":"10.1021/acs.est.4c12220","DOIUrl":"https://doi.org/10.1021/acs.est.4c12220","url":null,"abstract":"<i>N</i>-(1,3-Dimethylbutyl)-<i>N′</i>-phenyl-<i>p</i>-phenylenediamine-quinone (6PPD-Q), the tire rubber-derived transformation product of 6PPD, was recently discovered to cause the acute mortality of coho salmon (<i>Oncorhynchus kisutch</i>). Aiming to identify potential replacement antiozonants for 6PPD that do not produce toxic quinones, seven PPD-quinones with distinct side chains were synthesized to investigate their structure-related toxicities <i>in vivo</i> using rainbow trout (<i>Oncorhynchus mykiss</i>). While 6PPD-Q exerted high toxicity (96 h LC<sub>50</sub> = 0.35 μg/L), toxicity was not observed for six other PPD-quinones despite their similar structures. The fish tissue concentrations of 6PPD-Q after sublethal exposure (0.29 μg/L) were comparable to the other PPD-quinones, which indicated that bioaccumulation levels were not the reason for the selective toxicity of 6PPD-Q. Hydroxylated PPD-quinones were detected as the predominant metabolites in fish tissue. Interestingly, a single major aromatic hydroxylation metabolite was detected for the alternate PPD-quinones, but two abundant OH-6PPD-Q isomers were detected for 6PPD-Q. MS<sup>2</sup> spectra confirmed that hydroxylation occurred on the alkyl side chain for one isomer. The structurally selective toxicity of 6PPD-Q was also observed in a coho salmon (CSE-119) cell line, which further supports its intrinsic toxicity. This study reported the selective toxicity of 6PPD-Q and pinpointed the possibility for other PPDs to be applied as potential substitutes of 6PPD.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"38 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798194","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-08DOI: 10.1021/acs.est.5c0369610.1021/acs.est.5c03696
Julie Beth Zimmerman*, Gregory Lowry, Fernando Rosario-Ortiz, Paul Westerhoff, Daniel Alessi, Pedro Alvarez, Alexandra Boehm, Ian Cousins, Jordi Dachs, Matthew Eckelman, Imad El Haddad, Pablo Gago-Ferrero, Jorge Gardea-Torresdey, Jacqueline MacDonald Gibson, Keri Hornbuckle, Heileen Hsu-Kim, Juliane Hollender, Atsuko Ikeda, Frederic Leusch, Melissa Maurer-Jones, James Mihelcic, Shelly Miller, Lutgarde Raskin, Z. Jason Ren, Susan Richardson, Daniel Schlenk, Huahong Shi, Paul Tratnyek, David Waite, Shuxiao Wang, Zhanyun Wang, Michael Wong and Sukhwan Yoon,
Jian Sun, Zezhuang Liu, Fan Xia, Yilu Gu, Xiaofeng Gao, Sha Lu, Yang Xu, Feidan Meng, Qian Zhang, Tao Zhou
Rapid urbanization in China has exacerbated the urban heat island (UHI) effect, posing considerable challenges to urban sustainability and public health. Most UHI studies have focused on the impacts of two-dimensional (2D) urbanization, which involves outward city expansion and increased built-up area. However, as cities mature, they typically transition from horizontal expansion to vertical densification (3D urbanization), leading to increased material stock density. The implications of this shift for the UHI effect remain underexplored. This study compared the 2D and 3D urbanization–induced impacts on UHI across 384 Chinese cities from 2000 to 2020, using impervious surface and gridded material stocks. Our results surprisingly indicated that 2D urbanization lost explanatory power of the UHI intensity when the impervious surface area percentage exceeded 87%. Relative importance analysis utilizing a random forest algorithm revealed that the population, vegetation abundance, and precipitation significantly moderated the effects of 3D urbanization, emphasizing the crucial role of urban green spaces in mitigating thermal stress. This study examined the spatiotemporal dynamics of the UHI effect in China, emphasizing the key role of 3D urbanization. Our findings highlight the urgent need to incorporate 3D urbanization characteristics when devising UHI mitigation strategies.
{"title":"Uncovering the Impacts of 2D and 3D Urbanization on Urban Heat Islands in 384 Chinese Cities","authors":"Jian Sun, Zezhuang Liu, Fan Xia, Yilu Gu, Xiaofeng Gao, Sha Lu, Yang Xu, Feidan Meng, Qian Zhang, Tao Zhou","doi":"10.1021/acs.est.4c12689","DOIUrl":"https://doi.org/10.1021/acs.est.4c12689","url":null,"abstract":"Rapid urbanization in China has exacerbated the urban heat island (UHI) effect, posing considerable challenges to urban sustainability and public health. Most UHI studies have focused on the impacts of two-dimensional (2D) urbanization, which involves outward city expansion and increased built-up area. However, as cities mature, they typically transition from horizontal expansion to vertical densification (3D urbanization), leading to increased material stock density. The implications of this shift for the UHI effect remain underexplored. This study compared the 2D and 3D urbanization–induced impacts on UHI across 384 Chinese cities from 2000 to 2020, using impervious surface and gridded material stocks. Our results surprisingly indicated that 2D urbanization lost explanatory power of the UHI intensity when the impervious surface area percentage exceeded 87%. Relative importance analysis utilizing a random forest algorithm revealed that the population, vegetation abundance, and precipitation significantly moderated the effects of 3D urbanization, emphasizing the crucial role of urban green spaces in mitigating thermal stress. This study examined the spatiotemporal dynamics of the UHI effect in China, emphasizing the key role of 3D urbanization. Our findings highlight the urgent need to incorporate 3D urbanization characteristics when devising UHI mitigation strategies.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"108 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143789701","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jingyang Song, Xiaoke Su, Lijing Hou, Chunli Chu, Tongyuan Wu, Hancheng Dai, Yang Ou, Osamu Nishiura, Zhi Cao, Meiting Ju
In the global effort to mitigate climate change, the cement sector remains highly emission-intensive and hard-to-decarbonize. Previous research has highlighted material efficiency strategies─including more intensive use, lifetime extension, material-efficient design, and end-of-life processes, as demand-side options for reducing emissions. However, unintended effects and supply side responses, such as shifts in technological portfolios and investment trends, remain underexplored. This study develops a framework that couples detailed stock-flow modeling and a bottom-up energy system optimization model, a subcategory of integrated assessment models. Taking China’s cement sector as a pilot case, our framework projects comprehensive decarbonization pathways for cement-based materials. The results show that material efficiency strategies could reduce cement demand by 57%, significantly decreasing reliance on supply side technologies required for net-zero emissions, with these strategies contributing nearly 50% of the cumulative decarbonization effort. The material efficiency strategies also reduce the incremental total production costs associated with low-carbon technologies in upstream sectors. When combined with CO2 uptake from cement-based materials, this study offers a cost-effective pathway for achieving net-zero emissions in the cement sector, lowering both costs and CO2 emissions without heavy dependence on carbon capture and storage.
{"title":"Integrating Stock-Flow Modeling and Energy System Optimization to Explore Decarbonization Pathways for China’s Cement Industry","authors":"Jingyang Song, Xiaoke Su, Lijing Hou, Chunli Chu, Tongyuan Wu, Hancheng Dai, Yang Ou, Osamu Nishiura, Zhi Cao, Meiting Ju","doi":"10.1021/acs.est.4c14724","DOIUrl":"https://doi.org/10.1021/acs.est.4c14724","url":null,"abstract":"In the global effort to mitigate climate change, the cement sector remains highly emission-intensive and hard-to-decarbonize. Previous research has highlighted material efficiency strategies─including more intensive use, lifetime extension, material-efficient design, and end-of-life processes, as demand-side options for reducing emissions. However, unintended effects and supply side responses, such as shifts in technological portfolios and investment trends, remain underexplored. This study develops a framework that couples detailed stock-flow modeling and a bottom-up energy system optimization model, a subcategory of integrated assessment models. Taking China’s cement sector as a pilot case, our framework projects comprehensive decarbonization pathways for cement-based materials. The results show that material efficiency strategies could reduce cement demand by 57%, significantly decreasing reliance on supply side technologies required for net-zero emissions, with these strategies contributing nearly 50% of the cumulative decarbonization effort. The material efficiency strategies also reduce the incremental total production costs associated with low-carbon technologies in upstream sectors. When combined with CO<sub>2</sub> uptake from cement-based materials, this study offers a cost-effective pathway for achieving net-zero emissions in the cement sector, lowering both costs and CO<sub>2</sub> emissions without heavy dependence on carbon capture and storage.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"89 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143789703","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The property of groundwater dissolved organic matter (DOM) subjected to anthropogenic groundwater recharge (AGR) might be affected by the water quality disparity between surface water and natural groundwater. However, the diverse molecular scenarios of groundwater DOM under uneven recharging levels remain largely unexplored. We combined molecular characteristics, carbon isotopic signatures of organic molecules, and end-member mixing analysis to explore the sensitivity and potential tracking capabilities of DOM to AGR along with recharging gradients. Our findings suggested that AGR enriched groundwater with diverse, saturated, labile, and sulfur-rich molecules, amplifying DOM abundance and intensity, which intensified with recharge gradients. Additionally, S-containing molecules and their indicators like CHOS% (with threshold values of 7.82%) exhibited high sensitivity and predictive power for AGR recognition. The major signatures (diversity, saturated degree, and stability) indicated by 13C-containing molecules were similar to the whole molecular pool. Notably, specific molecules (C12H10O5S and C15H16O12), although not detected in all groundwater samples, exhibit robust stability or favorable solubility, rendering them potential candidates as AGR-sensitive molecules. The R13C/12C ratio of 13C-containing C19H24O5 emerged as the most robust tracer, exhibiting a strong correlation with the recharge ratio and the smallest deviation from the theoretical mixing line, signifying its optimal suitability for precise groundwater DOM source apportionment. This study offers novel insights into AGR impacts and contributes to fostering a harmonious balance between human activities and water resource sustainability.
{"title":"Carbon Isotopic Signatures of Aquifer Organic Molecules along Anthropogenic Recharge Gradients","authors":"Xu Cao, Wei He, Xian-Ge Wang, Xiaorui Chen, Bing Yi, Chao Ma, Xiaobo Li, Yu Liu, Wei He, Yuanyuan Shi","doi":"10.1021/acs.est.4c10929","DOIUrl":"https://doi.org/10.1021/acs.est.4c10929","url":null,"abstract":"The property of groundwater dissolved organic matter (DOM) subjected to anthropogenic groundwater recharge (AGR) might be affected by the water quality disparity between surface water and natural groundwater. However, the diverse molecular scenarios of groundwater DOM under uneven recharging levels remain largely unexplored. We combined molecular characteristics, carbon isotopic signatures of organic molecules, and end-member mixing analysis to explore the sensitivity and potential tracking capabilities of DOM to AGR along with recharging gradients. Our findings suggested that AGR enriched groundwater with diverse, saturated, labile, and sulfur-rich molecules, amplifying DOM abundance and intensity, which intensified with recharge gradients. Additionally, S-containing molecules and their indicators like CHOS% (with threshold values of 7.82%) exhibited high sensitivity and predictive power for AGR recognition. The major signatures (diversity, saturated degree, and stability) indicated by <sup>13</sup>C-containing molecules were similar to the whole molecular pool. Notably, specific molecules (C<sub>12</sub>H<sub>10</sub>O<sub>5</sub>S and C<sub>15</sub>H<sub>16</sub>O<sub>12</sub>), although not detected in all groundwater samples, exhibit robust stability or favorable solubility, rendering them potential candidates as AGR-sensitive molecules. The <i>R</i><sub>13C/12C</sub> ratio of <sup>13</sup>C-containing C<sub>19</sub>H<sub>24</sub>O<sub>5</sub> emerged as the most robust tracer, exhibiting a strong correlation with the recharge ratio and the smallest deviation from the theoretical mixing line, signifying its optimal suitability for precise groundwater DOM source apportionment. This study offers novel insights into AGR impacts and contributes to fostering a harmonious balance between human activities and water resource sustainability.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"74 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798197","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Guofang Xu, Haozheng He, Daoyu Tang, Qihong Lu, Bixian Mai, Zhili He, Lorenz Adrian, Jianzhong He, Jan Dolfing, Shanquan Wang
Polychlorinated biphenyls (PCBs) are pervasive pollutants that pose risks to ecosystems and human health. Microbial reductive dehalogenation plays crucial roles in attenuating PCBs, but comprehensive insights into PCB dechlorination pathways, reactivity, and governing factors are limited by the vast number of congeners and costly experimental approaches. We address this challenge by establishing a high-throughput in vitro assay approach of reductive dehalogenation (HINVARD), which increases dechlorination test throughput by 30-fold and enhances reagents and cell utilization efficiency by over 10-fold compared to conventional assay methods. Using HINVARD, we screened 61 PCB congeners across 9 enrichment cultures and 3 Dehalococcoides isolates, identifying active dechlorination of 31–44 congeners. Results showed that PCB congener properties (chlorine substitution patterns, steric hindrance, and solubility) primarily determine the dechlorination potential, leading to consistent reactivity trends across cultures. In contrast, different organohalide-respiring bacteria catalyzed distinct dechlorination pathways, preferentially removing para- or meta-chlorines. Structural modeling of reductive dehalogenases revealed unique binding orientations governing substrate specificity, offering molecular insights into these pathways. This study provides a high-efficiency strategy for investigating microbial reductive dehalogenation, yielding the first comprehensive understanding of PCB dechlorination patterns and mechanisms. These findings guide the design of tailored microbial consortia for effective PCB bioremediation.
{"title":"High-Throughput Screening of Microbial Reductive Dechlorination of Polychlorinated Biphenyls: Patterns in Reactivity and Pathways","authors":"Guofang Xu, Haozheng He, Daoyu Tang, Qihong Lu, Bixian Mai, Zhili He, Lorenz Adrian, Jianzhong He, Jan Dolfing, Shanquan Wang","doi":"10.1021/acs.est.4c13917","DOIUrl":"https://doi.org/10.1021/acs.est.4c13917","url":null,"abstract":"Polychlorinated biphenyls (PCBs) are pervasive pollutants that pose risks to ecosystems and human health. Microbial reductive dehalogenation plays crucial roles in attenuating PCBs, but comprehensive insights into PCB dechlorination pathways, reactivity, and governing factors are limited by the vast number of congeners and costly experimental approaches. We address this challenge by establishing a high-throughput <i>in vitro</i> assay approach of reductive dehalogenation (HINVARD), which increases dechlorination test throughput by 30-fold and enhances reagents and cell utilization efficiency by over 10-fold compared to conventional assay methods. Using HINVARD, we screened 61 PCB congeners across 9 enrichment cultures and 3 <i>Dehalococcoides</i> isolates, identifying active dechlorination of 31–44 congeners. Results showed that PCB congener properties (chlorine substitution patterns, steric hindrance, and solubility) primarily determine the dechlorination potential, leading to consistent reactivity trends across cultures. In contrast, different organohalide-respiring bacteria catalyzed distinct dechlorination pathways, preferentially removing <i>para</i>- or <i>meta</i>-chlorines. Structural modeling of reductive dehalogenases revealed unique binding orientations governing substrate specificity, offering molecular insights into these pathways. This study provides a high-efficiency strategy for investigating microbial reductive dehalogenation, yielding the first comprehensive understanding of PCB dechlorination patterns and mechanisms. These findings guide the design of tailored microbial consortia for effective PCB bioremediation.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"66 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798198","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kun Lin, Bo Li, Dong-Xing Guan, Zhiliang Wu, Xuezhen Li, Wenbing Ji, Wei Liu, Tao Yu, Zhongfang Yang
Natural manganese (Mn)-rich nodules effectively sequester cadmium (Cd) in soils and influence on the geochemical cycling of soil Cd, yet microscale understanding of their enrichment mechanisms remains limited. From a regional survey of 1448 rhizosphere soil-rice sample pairs in karst areas of Guangxi, China, we identified and characterized Mn-rich nodules from representative sites to investigate their role in Cd sequestration. Using chemical extractions combined with laser ablation–inductively coupled plasma–mass spectrometry (LA–ICP–MS) and X-ray photoelectron spectroscopy (XPS), we revealed that Mn oxides serve as primary Cd carriers in Mn-rich nodules, accounting for approximately 63.6% of total Cd, dominating Cd enrichment through binding mechanisms of Cd–O and Cd–OH bonds characteristic of inner-sphere surface complexation and structural incorporation. The stability of these chemical interactions was confirmed by pH-dependent experiments, showing <5.0% of total Cd release even at pH = 3.0. The high Mn(III) mass ratios (36.0%–40.0%) in nodules facilitated stable inner-sphere complexation, resulting in increased Cd retention. These study findings reveal the exceptional Cd sequestration capacity of natural Mn-rich nodules, and provide insights for the high concentrations and low availabilities of soil Cd in karst, which can aid in developing strategies for managing Cd-polluted karst soils.
{"title":"Enrichment Mechanisms of Cadmium in Natural Manganese-Rich Nodules from Karst Soils","authors":"Kun Lin, Bo Li, Dong-Xing Guan, Zhiliang Wu, Xuezhen Li, Wenbing Ji, Wei Liu, Tao Yu, Zhongfang Yang","doi":"10.1021/acs.est.4c11918","DOIUrl":"https://doi.org/10.1021/acs.est.4c11918","url":null,"abstract":"Natural manganese (Mn)-rich nodules effectively sequester cadmium (Cd) in soils and influence on the geochemical cycling of soil Cd, yet microscale understanding of their enrichment mechanisms remains limited. From a regional survey of 1448 rhizosphere soil-rice sample pairs in karst areas of Guangxi, China, we identified and characterized Mn-rich nodules from representative sites to investigate their role in Cd sequestration. Using chemical extractions combined with laser ablation–inductively coupled plasma–mass spectrometry (LA–ICP–MS) and X-ray photoelectron spectroscopy (XPS), we revealed that Mn oxides serve as primary Cd carriers in Mn-rich nodules, accounting for approximately 63.6% of total Cd, dominating Cd enrichment through binding mechanisms of Cd–O and Cd–OH bonds characteristic of inner-sphere surface complexation and structural incorporation. The stability of these chemical interactions was confirmed by pH-dependent experiments, showing <5.0% of total Cd release even at pH = 3.0. The high Mn(III) mass ratios (36.0%–40.0%) in nodules facilitated stable inner-sphere complexation, resulting in increased Cd retention. These study findings reveal the exceptional Cd sequestration capacity of natural Mn-rich nodules, and provide insights for the high concentrations and low availabilities of soil Cd in karst, which can aid in developing strategies for managing Cd-polluted karst soils.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"37 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143789704","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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